CN103367785B - A kind of all-vanadium flow battery and the method for operation thereof - Google Patents

A kind of all-vanadium flow battery and the method for operation thereof Download PDF

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CN103367785B
CN103367785B CN201310301519.9A CN201310301519A CN103367785B CN 103367785 B CN103367785 B CN 103367785B CN 201310301519 A CN201310301519 A CN 201310301519A CN 103367785 B CN103367785 B CN 103367785B
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electrolyte
vanadium
flow battery
additive
electrolyte liquid
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CN103367785A (en
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高新亮
张华民
王晓丽
刘若男
李颖
赵叶龙
林则青
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Dalian Rongke Power Co Ltd
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Dalian Rongke Power Co Ltd
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Priority to AU2014292587A priority patent/AU2014292587B2/en
Priority to EP14825952.6A priority patent/EP3024080B1/en
Priority to JP2016526430A priority patent/JP6231202B2/en
Priority to PCT/CN2014/082235 priority patent/WO2015007204A1/en
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
    • H01M8/184—Regeneration by electrochemical means
    • H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

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  • Fuel Cell (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)

Abstract

The present invention relates to a kind of its method of operation of all-vanadium flow battery, belong to flow battery field。A kind of all-vanadium flow battery, including anode electrolyte and electrolyte liquid, total vanadium ratio remains positive pole to described anode electrolyte with electrolyte liquid: negative pole is 1:1.5～1:1.2, and anode electrolyte and electrolyte liquid all contain additive, the concentration of additive is 0.01mol/L～0.5mol/L, wherein, described additive at least one in sulphuric acid, sulfate, phosphoric acid, phosphate, pyrophosphate, polyphosphate。The method both can keep high energy density to run, and can be substantially reduced again the irreversible decay of the discharge energy that liberation of hydrogen side reaction causes simultaneously。

Description

A kind of all-vanadium flow battery and the method for operation thereof
Technical field
The present invention relates to a kind of all-vanadium flow battery and the method for operation thereof, belong to flow battery field。
Background technology
As novel green secondary accumulator battery; all-vanadium flow battery (VFB) have have extended cycle life, advantage that easy scale, quickly response, addressing other battery systems such as freely hardly match, and successful Application in numerous large-sized solar energy storage and wind-powered electricity generation energy storage device and large-scale emergency power system and power system peak load shifting。
Electrolyte is critical material and the ergastic substances of vanadium cell, and in charging process, electrolyte is under left and right magnetic drive pump drives, and both positive and negative polarity solution, by ion-conductive membranes, following reaction occurs:
Positive pole reacts: VO2++H2O→VO2 ++2H++e-E0=1.00V...............(1)
Negative reaction: V3++e-→V2+E0=-0.26V................(2)
Evolving hydrogen reaction:
And in time being charged to a degree of, negative pole V2+Reach finite concentration to start and the H in electrolyte+There is evolving hydrogen reaction:
V2++H+→V3++H2↑ (3)
And this reaction directly results in negative pole and participates in the V of electric discharge2+Total amount reduces, and the discharge capacity of corresponding system reduces, and along with system is run, liberation of hydrogen side reaction is constantly accumulated and caused that both positive and negative polarity valence state is unbalance, will have a strong impact on the service efficiency of system, and the generation of hydrogen simultaneously also brings danger to environment。Problem above has become as vanadium cell and enters the technical bottleneck that practical stage is urgently to be resolved hurrily。
Safety in operation (additive):
The V when charging of positive solution is complete5+There is higher concentration (> 1M), in the case, when system is run more than 40 DEG C, very easily there is precipitation V in positive solution2O5↓。Precipitation will make electrode gap structure block, and cause systemic breakdown, strengthen battery maintenance cost。If taking cooling measure, then it is equipped with heat-exchange system and brings auxiliary facility cost and energy consumption to underestimate。
Now by adding a certain amount of additive in both positive and negative polarity solution to improve anode electrolyte operation stability more than 40 DEG C, it it is one of the problem that must solve。
The electrolyte stability additive of research both at home and abroad mainly had in recent years:
1) organic molecule class, such as glycerol, alcohols, organic acid, organic urea etc., research finds these machine thing molecules equal energy and V in positive solution5+There is redox reaction, by V5+It is reduced to V4+, itself is oxidized to CO2And water, lose stable V5+The ability of ion；
2) alkali metal sulfates, sodium sulfate, potassium sulfate, magnesium sulfate etc.；Existing many reports about alkali metal salt in document, but a certain amount of (> 2%, m/v need to be added) just effective, cause other concentration of metal ions in solution to raise, and there is no its pilot scale level at present and stablize the support of discharge and recharge application data。
Phosphoric acid and its esters have been reported that as V electrolyte stabilizer, but its add after the research of negative pole low-temperature stability still belong to blank, and stable storing test data under long-term extreme condition it is not yet reported that。
Europatent EP1143546 discloses a kind of all-vanadium flow battery method of operation, it is mentioned that increase UNICOM's pipeline by aligning negative solution storage tank upper end, slow down both positive and negative polarity vanadium solution and mutually migrate the system short term storage capability decline caused, but its irreversible capacity can not avoided the generation of liberation of hydrogen side reaction and cause declines, the improvement that significantly decays of its discharge capacity that system longtime running is caused is limited。
Summary of the invention
It is an object of the invention to provide a kind of all-vanadium flow battery。
A kind of all-vanadium flow battery, including anode electrolyte and electrolyte liquid, total vanadium ratio remains positive pole to described anode electrolyte with electrolyte liquid: negative pole is 1:1.5～1:1.2, and anode electrolyte and electrolyte liquid all contain additive, the concentration of additive is 0.01mol/L～0.5mol/L
Wherein, described additive at least one in sulphuric acid, sulfate, phosphoric acid, phosphate, pyrophosphate, polyphosphate。
Total vanadium amount of electrolyte is the concentration of vanadium ion × electrolyte volume in electrolyte；Total vanadium ratio refers to the ratio of total vanadium amount of anode electrolyte and total vanadium amount of electrolyte liquid to described anode electrolyte with electrolyte liquid；In described anode electrolyte, the concentration of vanadium ion is identical with the concentration of vanadium ion in electrolyte liquid；Described vanadium ion concentration includes the summation of the concentration of the vanadium ion of various valence states existing in electrolyte。
In prior art, anode electrolyte used in all-vanadium flow battery and electrolyte liquid are stored respectively in positive and negative electrode electrolyte storage tank, and total vanadium of anode electrolyte and electrolyte liquid is in equal proportions。Positive and negative electrode electrolyte is by VOSO4、V2(SO4)3In 1:0.5 ratio (i.e. V4+:V3+=1:1) configuration forms, and V4+: H2SO4Between 1:1.5-1:2。In time being charged to a degree of, negative pole V2+With the H in electrolyte when concentration is higher+There is evolving hydrogen reaction。Evolving hydrogen reaction and V in solution2+Concentration is positive correlation, i.e. V2+Concentration is more high, H2Produce speed more fast。Therefore, the present invention reduces the V of negative solution in cell operation2+Account for the total V of negative polen+The ratio (SOC state) of vanadium amount, namely takes to make negative pole total vanadium amount reduce V in electrolyte liquid more than a certain proportion of mode of positive pole2+Concentration。Practical operation by controlling both positive and negative polarity initial soln volume ratio, and can control the volume ratio of both positive and negative polarity electrolyte all the time in running, make the evolving hydrogen reaction of negative pole be preferably minimized, the capacity attenuation speed that the system that maintains is relatively low。It addition, the ratio of both positive and negative polarity electrolyte vanadium total amount can by transferring to realization in electrolyte liquid by anode electrolyte in running, the volume of the electrolyte of transfer is determined by the both positive and negative polarity vanadium ion concentration of the real time measure and the volume of both positive and negative polarity solution。
Remain that the total vanadium of positive pole and the total vanadium amount ratio of negative pole are 1:1.5～1:1.2, if after running multiple circulations, sampled detection, when the total vanadium amount of positive pole is close to negative pole amount, then by coupling cock, positive solution is derived a part and arrive negative pole, it is ensured that the ratio of the total vanadium amount of both positive and negative polarity is between 1:1.5～1:1.2。
That take above-mentioned measure simultaneously as the relative minimizing of anode volume so that positive solution is V when charging complete5+Ratio is up to more than 85% (normal state is about 60%), in the case, for avoiding positive solution because of V5+Excessive concentration or temperature are run more than 45 DEG C there is precipitation。Therefore, while controlling the full vanadium ratio of system, in anode electrolyte and electrolyte liquid, add additive, to suppress V in negative solution3+Precipitation under low temperature state, and suppress V in positive solution5+Precipitation at high temperature, it is achieved a kind of additive stablizes whole system。
The additive of all-vanadium flow battery of the present invention is at least one etc. in sulphuric acid, sulfate, phosphoric acid, phosphate, pyrophosphate, polyphosphate, and cation therein is preferably Na+。
Described additive preferably adds by following adding method in anode electrolyte and electrolyte liquid:
Electrolyte liquid: directly to doping in electrolyte liquid, the concentration making additive is 0.01mol/L～0.5mol/L, stirs after addition, to all dissolving mixing。
Anode electrolyte: first by additive dilute with water (additive: water is 1:1～1:4), adds the additive after dilution to anode electrolyte。
Additive can add under any temperature between-15 DEG C～55 DEG C。Wherein, polyphosphate addition is 0.01mol/L～0.5mol/L by monomer whose salt concentration in the electrolytic solution。
Total vanadium ratio remains positive pole to the preferred described anode electrolyte of all-vanadium flow battery of the present invention with electrolyte liquid: negative pole is 1:1.3～1:1.2。
The preferred described additive of all-vanadium flow battery of the present invention is phosphoric acid or phosphate。
The concentration of all-vanadium flow battery preferable additives of the present invention is 0.04～0.20mol/L, more preferably 0.20mol/L。
A kind of method of operation of all-vanadium redox flow battery system,
Total vanadium ratio remains positive pole to described anode electrolyte with electrolyte liquid: negative pole is 1:1.5～1:1.2, and the charging/discharging voltage scope that described all-vanadium flow battery runs is between 0.9V～1.58V。
It is preferred that described anode electrolyte is with electrolyte liquid, total vanadium ratio remains positive pole: negative pole is 1:1.3～1:1.2, and the charging/discharging voltage scope that described all-vanadium flow battery runs is between 0.9V～1.58V。
The discharge and recharge running temperature of the preferred described all-vanadium flow battery of the method for operation of all-vanadium redox flow battery system of the present invention is 0 DEG C～50 DEG C ,-20 DEG C～0 DEG C storage under fully charged state。
The flow battery of the different total vanadium method of salary distribution of the above-mentioned both positive and negative polarity provided, while avoiding power system capacity decay, it is (different according to total vanadium ratio that total discharge capacity (solution utilization rate) of system is subject to some effects, compared with initial both positive and negative polarity equivalent solution, total discharge capacity has the decline of about 20%), the method of operation expanding charging/discharging voltage scope is taken hence for this phenomenon, by conventional charge and discharge voltage 1.0V～1.55V, expand to 0.9V～1.58V, thus the problem that compensate for the electrolyte utilization rate decline that the total vanadium amount difference of both positive and negative polarity is brought。
The invention have the benefit that
The present invention proposes a kind of novel all-vanadium flow battery method of operation, namely the different total vanadium amount of both positive and negative polarity, change voltage range, use phosphoric acid class additive。The method both can keep high energy density to run, and can be substantially reduced again the irreversible decay of the discharge energy that liberation of hydrogen side reaction causes simultaneously。This method of operation is simple, does not increase any cost, is greatly improved the utilization rate of V electrolyte simultaneously, promotes battery performance, is suitable for industrialization promotion。
Accompanying drawing explanation
Fig. 1 is the volume change curve chart of embodiment 2 flow battery；
Fig. 2 is the volume change curve chart of embodiment 3 flow battery；
Fig. 3 is the volume change curve chart of embodiment 4 flow battery。
Detailed description of the invention
Following non-limiting example can make those of ordinary skill in the art more fully understand the present invention, but does not limit the present invention in any way。
Embodiment 1 is tested under high and low temperature, the Stabilization of phosphoric acid and additive salt thereof。
Embodiment 2～4 test battery used is respectively adopted Nafion115 type ionic membrane, and charging or discharging current density is 80mA/cm2When, small-sized 4w (48cm2Electrode area) monocell and 1.5kw (875cm2/ joint, 15 joints), battery pile is tested the battery performance of this method of operation and the common method of operation at 25 DEG C/40 DEG C/45 DEG C and is contrasted。In electrolyte, the concentration of vanadium ion is 1.55M。
Embodiment 1
The static storage experiment of phosphoric acid and sodium phosphate additive thereof
1.1 positive solution high temperature contrast experiments
Vanadium ion concentration is the pure pentavalent vanadium (V of 1.66M and 1.83M5+) electrolyte, in the airtight centrifuge tube of 10mL plastics。Adding phosphoric acid, content is 0.05M～0.3M, and compares test, in the water-bath of 40 DEG C and 50 DEG C, observes solution situation, and result of the test is shown in table 1 below。
The table 1 different additive addition Stabilization (precipitation natural law) to pentavalent vanadium solution
By data above it can be seen that for the electrolyte sample of same parameters, along with addition is different, its stabilization time is also different)。
1.2 low temperature storage tests:
Same method has investigated the effect to the low-temperature stability of trivalent vanadium solution of the above additive level at low temperatures。
Table 2 additive is to trivalent vanadium Stabilization (precipitation natural law) T=-20 DEG C at low temperatures
The low-temperature stability influence of trivalent vanadium is unidirectional by interpolation additive, and namely additive addition is more big, and low temperature stability inferior is more good。
Embodiment 2
Test parameters and result of the test are shown in following table, and volume change curve is shown in Fig. 1:
Embodiment 3
Test parameters and result of the test are shown in following table, and volume change curve is shown in Fig. 2:
Embodiment 4
Test parameters and result of the test are shown in following table, and volume change curve is shown in Fig. 3:

Claims (7)

1. an all-vanadium flow battery, including anode electrolyte and electrolyte liquid, it is characterised in that:
In described anode electrolyte and electrolyte liquid, total vanadium ratio remains positive pole: negative pole is 1:1.5～1:1.2, and all contains additive in anode electrolyte and electrolyte liquid, and the concentration of additive is 0.01mol/L～0.5mol/L,
Wherein, described additive at least one in sulphuric acid, sulfate, phosphoric acid, phosphate, pyrophosphate, polyphosphate。
2. battery according to claim 1, it is characterised in that: total vanadium ratio remains positive pole to described anode electrolyte with electrolyte liquid: negative pole is 1:1.3～1.2。
3. battery according to claim 1, it is characterised in that: described additive is phosphoric acid or phosphate。
4. battery according to claim 1, it is characterised in that: the concentration of additive is 0.04～0.2mol/L。
5. the method for operation of an all-vanadium redox flow battery system, it is characterised in that:
Total vanadium ratio remains positive pole to anode electrolyte with electrolyte liquid: negative pole is 1:1.5～1:1.2, and the charging/discharging voltage scope that described all-vanadium flow battery runs is between 0.9V～1.58V。
6. the method for operation according to claim 5, it is characterised in that:
Total vanadium ratio remains positive pole to described anode electrolyte with electrolyte liquid: negative pole is 1:1.3～1.2, and the charging/discharging voltage scope that described all-vanadium flow battery runs is between 0.9V～1.58V。
7. the method for operation according to claim 5 or 6, it is characterised in that: the discharge and recharge running temperature of described all-vanadium flow battery is 0 DEG C～50 DEG C ,-20 DEG C～45 DEG C storages under fully charged state。
CN201310301519.9A 2013-07-17 2013-07-17 A kind of all-vanadium flow battery and the method for operation thereof Active CN103367785B (en)

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CN201310301519.9A CN103367785B (en) 2013-07-17 2013-07-17 A kind of all-vanadium flow battery and the method for operation thereof
AU2014292587A AU2014292587B2 (en) 2013-07-17 2014-07-15 All-vanadium redox flow battery and operation method thereof
EP14825952.6A EP3024080B1 (en) 2013-07-17 2014-07-15 All-vanadium redox flow battery and operation method thereof
JP2016526430A JP6231202B2 (en) 2013-07-17 2014-07-15 All vanadium redox flow battery and operation method thereof
PCT/CN2014/082235 WO2015007204A1 (en) 2013-07-17 2014-07-15 All-vanadium redox flow battery and operation method thereof

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WO2015007204A1 (en) 2015-01-22
AU2014292587A1 (en) 2016-02-11
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